An eruption of Italian volcano Mount Etna on 3 December 2015 produced fast-moving sulfur dioxide (SO2) and sulfate aerosol clouds that traveled across Asia and the Pacific Ocean, reaching North America in just 5 days. The Ozone Profiler and Mapping Suite’s Nadir Mapping UV spectrometer aboard the U.S. National Polar-orbiting Partnership satellite observed the horizontal transport of the SO2 cloud. Vertical profiles of the colocated volcanic sulfate aerosols were observed between 11.5 and 13.5 km by the new Cloud Aerosol Transport System (CATS) space-based lidar aboard the International Space Station. Backward trajectory analysis estimates the SO2 cloud altitude at 7–12 km. Eulerian model simulations of the SO2 cloud constrained by CATS measurements produced more accurate dispersion patterns compared to those initialized with the back trajectory height estimate. The near-real-time data processing capabilities of CATS are unique, and this work demonstrates the use of these observations to monitor and model volcanic clouds.